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Importance of Zinc Oxide in Cu-Based Catalysts for the Ethynylation of Formaldehyde to 1,4-Butynediol | |
BSRF用户 | |
2021 | |
Source Publication | JOURNAL OF PHYSICAL CHEMISTRY C
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ISSN | 1932-7447 |
EISSN | 1932-7455 |
Volume | 125Issue:30Pages:16536--16549 |
Subtype | Article |
Abstract | As more technologies have been developed to produce formaldehyde and acetylene from biomass, the condensation-addition reaction between formaldehyde and acetylene provides a green and atom-economic method to synthesize 1,4-butynediol (BD). It is important to design and construct a new efficient copper-based catalyst for formaldehyde ethynylation with multi-center synergy to improve the reaction efficiency. In this work, a CuO-xZnO composite catalyst with an interface structure was constructed. Compared with a CuO-based catalyst, the yield of BD was increased from 19.07 to 70.9% by introducing an appropriate amount of ZnO, and the reaction activation energy decreased from 28.94 to 16.35 kJ/mol, which improved the catalytic reaction efficiency. The results showed that ZnO in the CuO-xZnO catalyst dispersed the active Cu species and also promoted the conversion of CuO to copper acetylide by electron transfer in the interface structure. Moreover, Zn2+ in ZnO acted as a Lewis acid and adsorbed the carbonyl oxygen of formaldehyde, causing the carbonyl electrons to flow to Zn2+, which enhanced the electropositivity of C+ in the formaldehyde molecule. This resulted in a nucleophilic addition reaction between formaldehyde activated by ZnO and acetylene activated by copper acetylide at the interface, which efficiently generated the target product BD. |
DOI | 10.1021/acs.jpcc.1c04886 |
Indexed By | SCI |
Language | 英语 |
WOS Research Area | Chemistry ; Science & Technology - Other Topics ; Materials Science |
WOS Subject | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
WOS ID | WOS:000683810700020 |
ItemNo | BSRF00524 |
beamline | 1W1B |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.ihep.ac.cn/handle/311005/293292 |
Collection | 北京同步辐射装置 |
Recommended Citation GB/T 7714 | BSRF用户. Importance of Zinc Oxide in Cu-Based Catalysts for the Ethynylation of Formaldehyde to 1,4-Butynediol[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2021,125(30):16536--16549. |
APA | BSRF用户.(2021).Importance of Zinc Oxide in Cu-Based Catalysts for the Ethynylation of Formaldehyde to 1,4-Butynediol.JOURNAL OF PHYSICAL CHEMISTRY C,125(30),16536--16549. |
MLA | BSRF用户."Importance of Zinc Oxide in Cu-Based Catalysts for the Ethynylation of Formaldehyde to 1,4-Butynediol".JOURNAL OF PHYSICAL CHEMISTRY C 125.30(2021):16536--16549. |
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